AU2015349218B2 - Quinone polyhalide flow battery - Google Patents

Quinone polyhalide flow battery Download PDF

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AU2015349218B2
AU2015349218B2 AU2015349218A AU2015349218A AU2015349218B2 AU 2015349218 B2 AU2015349218 B2 AU 2015349218B2 AU 2015349218 A AU2015349218 A AU 2015349218A AU 2015349218 A AU2015349218 A AU 2015349218A AU 2015349218 B2 AU2015349218 B2 AU 2015349218B2
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electrolyte
negative
flow battery
quinone
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Yuanhui CHENG
Qinzhi LAI
Xianfeng Li
Chenhui Wang
Huamin Zhang
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Dalian Institute of Chemical Physics of CAS
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
    • H01M8/184—Regeneration by electrochemical means
    • H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0569—Liquid materials characterised by the solvents
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/96—Carbon-based electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/20—Indirect fuel cells, e.g. fuel cells with redox couple being irreversible
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
    • H01M2004/8684—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
    • H01M2004/8689—Positive electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0002—Aqueous electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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  • General Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
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Abstract

A quinone polyhalide flow battery, where the positive electrode electrolyte is a solution of hydrochloric acid mixed with sodium sulfide, and the negative electrode electrolyte is a solution of hydrochloric acid mixed with anthraquinone. This improves the problem of high costs and low battery voltage of an anthraquinone flow battery.

Description

QUINONE POLYHALIDE FLOW BATTERY
Technical Field
The present invention relates to a flow battery system.
Background
Recently, with the increasing shortage of the world's energy supply, the development and utilization of wind energy, solar energy and other renewable energy attract much attention. But
the efficient, cheap, safe and reliable energy storage technologies must be combined with the renewable energy in order to ensure the steady power supply of solar, wind and other renewable energy power generation systems. Among various energy storage technologies, the flow energy storage battery, one chemical energy storage method, becomes one of the most suitable batteries for large-scale energy storage at present because of unique advantages.
Now, two kinds of well-developed flow battery systems are vanadium flow battery and zinc bromine flow battery. The vanadium flow battery realizes the reversible conversion between the chemical energy and electric energy by an electrochemical reaction of vanadium ions with different valence states in the electrolyte on an inert electrode. The positive and negative redox couples are VO+/VO2+ and V2+N 3 * respectively. The sulfuric acid acts as a supporting electrolyte. Because of the vanadium ions with different valence states on the positive and negative sides, the contamination caused by the movement of each other to the electrolyte is avoided and the battery performance and life are improved. In addition, a vanadium electrolyte can be easily recovered, thereby further improving the life of a battery system and reducing operating costs. But the electrolyte cost of the vanadium flow battery and the cost of a proton exchange membrane are relatively high, and a certain cross contamination problem exists in the positive and negative electrolyte. .
The positive and negative half-battery of the zinc bromine flow battery is separated by a separator, and the electrolytes on both sides are ZnBr2 solution. Under the action of a power pump, the electrolyte conducts circular flow in a closed loop composed of a reservoir and a battery. The main problem that the zinc bromine flow battery exists is the bromine contamination.
The quinone bromine flow battery has been reported in a literature, but since a proton exchange membrane is used in the literature, and the sulfuric acid is used as the supporting electrolyte, the cost and battery voltage are low. The present invention uses a porous membrane and uses the hydrochloric acid as the supporting electrolyte, so that the cost is reduced while the voltage is increased.
Summary In one aspect, the present invention provides a a quinone polyhalide flow battery comprising a battery module, a reservoir reserving positive electrolyte, a reservoir reserving negative electrolyte, a circulating pump and pipes, wherein the battery module is formed by two, three or more than three sections of single cells in series and each single cell includes a positive electrode, a separator and a negative electrode, wherein the positive electrolyte is a mixed solution of hydrochloric acid and sodium bromide and the negative electrolyte is a mixed solution of hydrochloric acid and anthraquinone, and wherein the positive and negative electrolytes contain 0.1-1 M of quaternary ammonium salt molecular bromine complexing agents.
In another aspect the present invention provides quinone polyhalide flow battery system, comprising: a positive end plate, a negative end plate, a positive electrode, a porous membrane, a negative electrode, a reservoir, pipes and pumps. Wherein the positive and negative electrodes consist of a current collector and catalytic materials; and during the charging and discharging processes, the electrolyte are transported to the positive and negative electrodes from the reservoir via the pump(s), and redox reactions of bromine ion/molecular bromine and quinone/anthraquinone occur on the positive and negative electrodes respectively.
The present invention provides a quinone polyhalide flow battery. In some embodiments, the battery consists of a battery module, an electrolyte reservoir reserving positive electrolyte, an electrolyte reservoir reserving negative electrolyte, a circulating pump and pipes, wherein the battery module may be formed by two, three or more than three sections of single cells in series, and the single cell includes a positive electrode, a separator, and a negative electrode. The positive electrolyte may be a mixed solution of hydrochloric acid and sodium bromide and the negative electrolyte may be a mixed solution of hydrochloric acid and anthraquinone.
The positive electrolyte may be a mixed solution of 0.5-2 M of hydrochloric acid and 0.5-2M of sodium bromide. The negative electrolyte may be a mixed solution of 0.5-2M of hydrochloric acid and 0.5-IM of anthraquinone.
The positive and negative electrolytes contain 0.1-1 M of quaternary ammonium salt molecular bromine complexing agents, which interacts with the molecular bromine to form molecular bromine complex, to realize the phase separation of electrolyte and reduce the molecular bromine diffusion.
The quaternary ammonium salt molecular bromine complexing agent may be N methylethylpyrrolidinium bromide (MEP) or N-methylethyl morpholinium bromide (MEM). The positive and negative materials are activated carbon felt. The separator may be a porous membrane or a dense membrane. Single cell includes a positive end plate, a positive electrode, a separator, a negative electrode and a negative end plate.
The beneficial effects of the present invention:
This patent proposes a concept of quinone polyhalides flow battery by improving the technology, so that the problems that the cost of a quinone bromine flow battery may be relatively high and the voltage of the battery may be relatively low are improved.
Brief Description of the Drawings
Figure 1 is the battery cycle stability diagram of example 1; Figure 2 is the battery cycle stability of comparative example 1; Figure 3 is the comparison curve diagram of battery charge and discharge of example 1 and comparative example 1.
Detailed Description of the Embodiments 100
The porous membrane is adopted to assemble the batteries in examples and comparative examples, unless otherwise specified.
105 Example 1 Electrolyte preparation and battery assembly: Positive electrolyte: 40 mLof 1 M HCl + 0.5 M N-methylethylpyrrolidinium bromide + 1 M sodium bromide; Negative electrolyte: 40 mL of IM HCl + 0.5M N-methylethylpyrrolidinium bromide + IM 110 anthraquinone solution. Single cell is assembled by a positive end plate, a positive electrode 22 3x3cm,a carbon felt, membrane, a carbon felt, a negative electrode graphite plate 3x3cm2 and a negative end plate in turn.
Battery Test: 115 Electrolyte flow rate: 5mL/min; Charge-discharge current density: 20 mA/cm 2; The cycle stability of battery is shown in Figure 1.
Comparative example 1 Electrolyte preparation and battery assembly: 120 Positive electrolyte: 40 mL of 0.5 M H 2 SO4 + 1 M sodium bromide; Negative electrolyte: 40 mL of 0.5 M H2 SO4 + IM anthraquinone solution. Single cell is assembled by a positive end plate, a positive electrode 3x3cm2 , a carbon felt, membrane, a carbon felt, a negative electrode graphite plate 3x3cm2 and a negative end plate in turn. Battery Test: 125 Electrolyte flow rate: 5mL/min; Charge-discharge current density: 20 mA/cm 2 ; the cycle stability of battery is shown in Figure 1.
A comparison curve of battery charge and discharge of example 1 and comparative example 1 is shown in Figure 3. 130
The present invention relates to a quinone polyhalide flow battery, comprising: a positive end plate, a negative end plate, a positive electrode, a porous membrane, a negative electrode, a reservoir, pipes and pumps. Wherein the positive and negative electrodes consist of a current collector and catalytic materials of positive and negative electrodes; and during the charging 135 and discharging processes, the electrolyte is transported to the positive and negative electrodes from the reservoir via the pump, and redox reactions of bromine ion/molecular bromine and quinone/anthraquinone occurr on the positive and negative electrodes respectively.
As shown in Figure. 2 and 3: the charge voltage has decreased and the discharge voltage has 140 increased by adopting HCl as supporting electrolyte. In addition, the battery performance is improved, and the cycle performance is better than those of the battery which adopts H 2 SO4 as electrolyte.
In an optimized condition, unless stated, the volumes of positive and negative electrolyte are 145 40 mL. Single cell is assembled by a positive end plate, a positive electrode 3x3cm2 , a carbon felt, membrane, a carbon felt, a negative electrode graphite plate 3x3cm2 and a negative end plate in turn. In a battery test, the electrolyte flow rate is 5 mL/min; and the charge-discharge current density is 20 mA/cm 2 . The battery performances are shown in tables 1 and 2.
150 It can be seen from the preferred result that the battery performance increases with the increasing of the HCl concentration in positive electrolyte and keeps stable until the HCl concentration attained 1.0 mol/L. The battery performance increases and keeps stable with the increasing of the concentration of sodium bromide in positive electrolyte. In order to improve the battery energy density, the concentrations of HCl and sodium bromide in positive 155 electrolyte are 2 mol/L. The HCl concentration in negative electrolyte is finally selected as 2 mol/L to keep the same as that of the positive electrolyte. However, the increasing concentration of quinone is detrimental to the improvement of the battery performance, thus the concentration of quinone is finally preferably selected as 0.5 mol/L. It can be seen from the comparison that the addition of MEP can significantly improve the battery performance 160 and possess better effects than MEM. However too much addition of the complexing agent will increase the cost in one aspect and also decrease the battery performance in another aspect, thus the concentration is preferably selected as 0.5 mol/L.
The final optimizing conditions of the electrolyte are various concentration parameters as 165 shown in No. 7.
Table 1 Sodium HCl bromide HCl Quinone Concentratio concentratio concentratio concentratio concentratio Types of n of n in positive n in positive n in negative n in negative complexin complexing Types of No. electrolyte electrolyte electrolyte electrolyte g agent agent membrane (mol/L) (mol/L) (mol/L) (mol/L) (mol/L) microporous 1 0.5 0.5 0.5 0.5 MEP 0.1 membrane
microporous 2 1.0 1.0 0.5 0.5 MEP 0.1 membrane
microporous 3 2.0 2.0 0.5 0.5 MEP 0.1 membrane
microporous 4 2.0 2.0 1.0 0.5 MEP 0.1 membrane
microporous 5 2.0 2.0 2.0 0.5 MEP 0.1 membrane
microporous 6 2.0 2.0 2.0 1 MEP 0.1 membrane
microporous 7 2.0 2.0 2.0 0.5 MEP 0.5 membrane
microporous 8 2.0 2.0 2.0 0.5 MEP 1.0 membrane
microporous 9 2.0 2.0 2.0 0.5 MEM 0.1 membrane
microporous 10 2.0 2.0 2.0 0.5 MEM 0.5 membrane
microporous 11 2.0 2.0 2.0 0.5 MEM 1.0 membrane
12 2.0 2.0 2.0 0.5 MEP 1.0 Nafion 115
13 2.0 2.0 2.0 0.5 MEP 1.0 Nafion 117
170
5a
175 Table 2 Voltage efficiency Number Coulombic efficiency(%) (%) Energy efficiency (%) 1 96 83 80
2 96 85 82
3 96 84 81
4 96 86 83
5 96 85 82
6 96 85 82
7 97 86 83
8 98 83 81
9 94 85 80
10 96 85 82
11 97 80 78
12 99 81 80
13 99 80 79
Throughout this specification and the claims which follow, unless the context requires otherwise, the word "comprise", and variations such as "comprises" and "comprising", will be 180 understood to imply the inclusion of a stated integer or step or group of integers or steps but not the exclusion of any other integer or step or group of integers or steps.
The reference in this specification to any prior publication (or information derived from it), or to any matter which is known, is not, and should not be taken as an acknowledgment or 185 admission or any form of suggestion that that prior publication (or information derived from it) or known matter forms part of the common general knowledge in the field of endeavour to which this specification relates.
5b

Claims (7)

The claims defining the invention are as follows:
1. A quinone polyhalide flow battery comprising a battery module, a reservoir reserving positive electrolyte, a reservoir reserving negative electrolyte, a circulating pump and pipes, wherein the battery module is formed by two, three or more than three sections of single cells in series and each single cell includes a positive electrode, a separator and a negative electrode, wherein the positive electrolyte is a mixed solution of hydrochloric acid and sodium bromide and the negative electrolyte is a mixed solution of hydrochloric acid and anthraquinone, and wherein the positive and negative electrolytes contain 0.1-1 M of quaternary ammonium salt molecular bromine complexing agents.
2. The quinone polyhalide flow battery according to claim 1, wherein the positive electrolyte is a mixed solution of 0.5-2 M of hydrochloric acid and 0.5-2 M of sodium bromide.
3. The quinone polyhalide flow battery according to claim 1 or 2, wherein the negative electrolyte is a mixed solution of 0.5-2 M of hydrochloric acid and 0.5-iM of anthraquinone.
4. The quinone polyhalide flow battery according to any one of claims I to 3, wherein the quaternary ammonium salt molecular bromine complexing agent is N-methylethylpyrrolidinium bromide (MEP) orN-methylethyl morpholinium bromide.
5. The quinone polyhalide flow battery according to any one of claims 1 to 4, wherein the positive and negative electrode materials are activated carbon felt.
6. The quinone polyhalide flow battery according to any one of claims I to 5, wherein the separator is a porous membrane or a dense membrane.
7. The quinone polyhalide flow battery according to any one of claims 1 to 6, wherein each single cell includes a positive end plate, a positive electrode, a separator, a negative electrode and a negative end plate.
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CN201410653131.XA CN105679985B (en) 2014-11-17 2014-11-17 A kind of quinone polyhalide flow battery
PCT/CN2015/092059 WO2016078492A1 (en) 2014-11-17 2015-10-16 Quinone polyhalide flow battery

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EP3223354B1 (en) 2019-11-13
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JP2017517101A (en) 2017-06-22
JP6247778B2 (en) 2017-12-13
US20170025700A1 (en) 2017-01-26
AU2015349218A1 (en) 2016-11-03
EP3223354A4 (en) 2018-07-04
CN105679985A (en) 2016-06-15
WO2016078492A1 (en) 2016-05-26
US10446867B2 (en) 2019-10-15

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